Interfacing with Fe-N-C Sites Boosts the Formic Acid Dehydrogenation of Palladium Nanoparticles

Hierarchical micro-/mesoporous carbons with abundant Fe-N-C sites were prepared through one-step carbonization of a metal-organic framework (MOF) with sodium iron ethylenediaminetetraacetic acid [NaFe(III)EDTA], which can facilitate the nucleation and growth of ultrafine (∼1.4 nm) and highly dispersed palladium nanoparticles (Pd NPs). Interfacing Pd NPs with Fe-N-C sites has been demonstrated for the first time to boost the heterogeneous catalysis of hydrogen production from formic acid, affording an ultrahigh turnover frequency (TOF) value of 7361 h^-1 at 323 K. The robust synergistic interactions between Pd NPs and Fe-N-C sites together with the small size effects of Pd NPs are responsible for the enhanced catalytic activity.